Cited by 566Spectroscopy and Quantum Chemical StudiesPhotochemistry and Electron Transfer StudiesPhotosynthetic Processes and Mechanisms

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Electronic resonance with anticorrelated pigment vibrations drives photosynthetic energy transfer outside the adiabatic framework

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Tiwari, Vivek, Peters, William K., Jonas, David M.·2013·Proceedings of the National Academy of Sciences

DOI 10.1073/pnas.1211157110PMC PMC3557059

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Abstract

The delocalized, anticorrelated component of pigment vibrations can drive nonadiabatic electronic energy transfer in photosynthetic light-harvesting antennas. In femtosecond experiments, this energy transfer mechanism leads to excitation of delocalized, anticorrelated vibrational wavepackets on the ground electronic state that exhibit not only 2D spectroscopic signatures attributed to electronic coherence and oscillatory quantum energy transport but also a cross-peak asymmetry not previously explained by theory. A number of antennas have electronic energy gaps matching a pigment vibrational frequency with a small vibrational coordinate change on electronic excitation. Such photosynthetic energy transfer steps resemble molecular internal conversion through a nested intermolecular funnel.

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Authors: Tiwari, V., Peters, W. K., & Jonas, D. M.
Affiliations: University of Colorado Boulder (US)
ORCID: Tiwari, Vivek
Peters, William K.
Jonas, David M.
Venue: Proceedings of the National Academy of Sciences
Publisher: National Academy of Sciences
Published: 2012-12-24
Volume: 110
Issue: 4
Pages: 1203-1208
ISSN: 0027-8424 (ISSN-L)
1091-6490
DOI: 10.1073/pnas.1211157110
PMC: PMC3557059
OpenAlex: W2066289545
Cited by: 566
References: 36
Citations by year: 2026: 21 · 2025: 33 · 2024: 29 · 2023: 42 · 2022: 31 · 2021: 29 · 2020: 34 · 2019: 49 · 2018: 50 · 2017: 57 · 2016: 42 · 2015: 55 · 2014: 50 · 2013: 41
FWCI: 24.13
Type: journal article
Language: en
Open access: bronze
doi.org
Locations: Proceedings of the National Academy of Sciences (publishedVersion)
Europe PMC (PubMed Central) (publishedVersion)
PubMed Central (publishedVersion)
PubMed (publishedVersion)
Funders: National Science Foundation (1112365, 0821794)
National Center for Atmospheric Research (CNS-0821794)
University of Colorado Boulder (CNS-0821794)
University of Colorado Denver (CNS-0821794)
Division of Chemistry (CHE-1112365)
Topics: Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Biology › Photosynthetic Processes and Mechanisms
Keywords: photosynthetic energy transfer, vibrational wave packets, 2D spectroscopy, electronic coherence, light-harvesting antenna, internal conversion
MeSH terms: Electron Transport, Electrons, Energy Transfer, Models, Biological, Photosynthesis, Quantum Theory, Spectrum Analysis, Vibration, Photosynthetic Reaction Center Complex Proteins

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Electronic resonance with anticorrelated pigment vibrations drives photosynthetic energy transfer outside the adiabatic framework

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